基于氨气回收柔性金属有机骨架材料结构重建快速再生机理研究

氨既是粮食能源（氮肥）又是雾霾推手，回收直排低浓度氨气兼具资源化再利用和降低大气污染的双重目的。吸附法具有氨气回收过程无相变，直接与二氧化碳反应合成氮肥（如尿素）的优势。基于柔性金属有机骨架材料（MOFs）Cu(INA)2所具有的氨气吸附量大及固氨特性，作为氨气回收吸附剂优势明显。柔性的Cu(INA)2在脱氨后拓扑结构重新组建所需时间较长，存在吸附剂再生速率慢的问题，限制了其工业应用。本项目创新性的提出利用引入类水极性分子吹扫脱氨后的柔性片段（金属和异烟酸）形成过渡态来达到促进原始拓扑结构重建的目的，实现吸附剂的快速再生。深入研究Cu(INA)2吸脱附气体后的结构转变机理，无氨气时柔性片段的自组装记忆效应，氨气在柔性MOFs中的吸附热力学与动力学性质以及吸附剂的循环捕集氨气效果，为直排低浓度氨气高效回收提供可以快速再生的可逆吸附剂，为拓展柔性MOFs材料的工业应用奠定基础。

Ammonia has two sides, useful side: energy of grain, harmful side: haze push. Recycling of low concentrations ammonia from the atmosphere has dual purpose: resource recycling and air pollution reducing. Ammonia adsorption process with no phase change, then, the enriched ammonia can be directly synthesized nitrogen fertilizer (urea) with carbon dioxide. Based on the ammonia-fixing characteristics of flexible metal-organic frameworks (MOFs) Cu(INA)2 with the structure changed to steady state after large ammonia adsorbing, we will chose Cu(INA)2 as the recycling ammonia adsorbent in this project. However, too long time needed for the structure reconstituted, so the adsorbent regeneration is the key issue. Innovative proposed to achieve the original topology reconstruction purpose by the formation of transition state used a class of polar water molecules purging way, realize rapid regeneration of the adsorbent. Deeply understand the structural transition mechanism of Cu(INA)2 after ammonia adsorption-desorption, the memory of self-assembly for the flexible segment with no ammonia adsorbed, the thermodynamic and kinetic properties of ammonia adsorption, and cycle ammonia capture effect of adsorbents. Provide fast reversible regeneration adsorbent material for recycling low concentration ammonia from direct emissions air pollutants, and lay the foundation for expanding the industrial application of flexible MOFs materials.